Rashba-like Spin Textures in Graphene Promoted by Ferromagnet-Mediated Electronic Hybridization with a Heavy Metal.

Epitaxial graphene/ferromagnetic metal (Gr/FM) heterostructures deposited onto heavy metals have been proposed for the realization of spintronic devices because of their perpendicular magnetic anisotropy and sizable Dzyaloshinskii-Moriya interaction (DMI), allowing for both enhanced thermal stability and stabilization of chiral spin textures. However, establishing routes toward this goal requires the fundamental understanding of the microscopic origin of their unusual properties. Here, we elucidate the nature of the induced spin-orbit coupling (SOC) at Gr/Co interfaces on Ir. Through spin- and angle-resolved photoemission spectroscopy along with density functional theory, we show that the interaction of the heavy metals with the Gr layer via hybridization with the FM is the source of strong SOC in the Gr layer. Furthermore, our studies on ultrathin Co films underneath Gr reveal an energy splitting of ∼100 meV for in-plane and negligible for out-of-plane spin polarized Gr π-bands, consistent with a Rashba-SOC at the Gr/Co interface, which is either the fingerprint or the origin of the DMI. This mechanism vanishes at large Co thicknesses, where neither in-plane nor out-of-plane spin-orbit splitting is observed, indicating that Gr π-states are electronically decoupled from the heavy metal. The present findings are important for future applications of Gr-based heterostructures in spintronic devices.

Temperature Dependence of Relativistic Valence Band Splitting Induced by an Altermagnetic Phase Transition.

Altermagnetic (AM) materials exhibit non-relativistic, momentum-dependent spin-split states, ushering in new opportunities for spin electronic devices. While the characteristics of spin-splitting are documented within the framework of the non-relativistic spin group symmetry, there is limited exploration of the inclusion of relativistic symmetry and its impact on the emergence of a novel spin-splitting in the band structure. This study delves into the intricate relativistic electronic structure of an AM material, α-MnTe. Employing temperature-dependent angle-resolved photoelectron spectroscopy across the AM phase transition, the emergence of a relativistic valence band splitting concurrent with the establishment of magnetic order is elucidated. This discovery is validated through disordered local moment calculations, modeling the influence of magnetic order on the electronic structure and confirming the magnetic origin of the observed splitting. The temperature-dependent splitting is ascribed to the advent of relativistic spin-splitting resulting from the strengthening of AM order in α-MnTe as the temperature decreases. This sheds light on a previously unexplored facet of this intriguing material.

Inducing Single Spin-Polarized Flat Bands in Monolayer Graphene.

Due to the fundamental and technological implications in driving the appearance of non-trivial, exotic topological spin textures and emerging symmetry-broken phases, flat electronic bands in 2D materials, including graphene, are nowadays a relevant topic in the field of spintronics. Here, via europium doping, single spin-polarized bands are generated in monolayer graphene supported by the Co(0001) surface. The doping is controlled by Eu positioning, allowing for the formation of a K ¯ $\bar{\mathrm{K}}$ -valley localized single spin-polarized low-dispersive parabolic band close to the Fermi energy when Eu is on top, and of a π* flat band with single spin character when Eu is intercalated underneath graphene. In the latter case, Eu also induces a bandgap opening at the Dirac point while the Eu 4f states act as a spin filter, splitting the π band into two spin-polarized branches. The generation of flat bands with single spin character, as revealed by the spin- and angle-resolved photoemission spectroscopy (ARPES) experiments, complemented by density functional theory (DFT) calculations, opens up new pathways toward the realization of spintronic devices exploiting such novel exotic electronic and magnetic states.

Visualizing Higher-Fold Topology in Chiral Crystals.

Novel topological phases of matter are fruitful platforms for the discovery of unconventional electromagnetic phenomena. Higher-fold topology is one example, where the low-energy description goes beyond standard model analogs. Despite intensive experimental studies, conclusive evidence remains elusive for the multigap topological nature of higher-fold chiral fermions. In this Letter, we leverage a combination of fine-tuned chemical engineering and photoemission spectroscopy with photon energy contrast to discover the higher-fold topology of a chiral crystal. We identify all bulk branches of a higher-fold chiral fermion for the first time, critically important for allowing us to explore unique Fermi arc surface states in multiple interband gaps, which exhibit an emergent ladder structure. Through designer chemical gating of the samples in combination with our measurements, we uncover an unprecedented multigap bulk boundary correspondence. Our demonstration of multigap electronic topology will propel future research on unconventional topological responses.

Coexistence of Bulk-Nodal and Surface-Nodeless Cooper Pairings in a Superconducting Dirac Semimetal.

The interplay of nontrivial topology and superconductivity in condensed matter physics gives rise to exotic phenomena. However, materials are extremely rare where it is possible to explore the full details of the superconducting pairing. Here, we investigate the momentum dependence of the superconducting gap distribution in a novel Dirac material PdTe. Using high resolution, low temperature photoemission spectroscopy, we establish it as a spin-orbit coupled Dirac semimetal with the topological Fermi arc crossing the Fermi level on the (010) surface. This spin-textured surface state exhibits a fully gapped superconducting Cooper pairing structure below T_{c}∼4.5 K. Moreover, we find a node in the bulk near the Brillouin zone boundary, away from the topological Fermi arc. These observations not only demonstrate the band resolved electronic correlation between topological Fermi arc states and the way it induces Cooper pairing in PdTe, but also provide a rare case where surface and bulk states host a coexistence of nodeless and nodal gap structures enforced by spin-orbit coupling.

Ferromagnetic Layers in a Topological Insulator (Bi,Sb)2Te3 Crystal Doped with Mn.

Magnetic topological insulators (MTIs) have recently become a subject of poignant interest; among them, Z2 topological insulators with magnetic moment ordering caused by embedded magnetic atoms attract special attention. In such systems, the case of magnetic anisotropy perpendicular to the surface that holds a topologically nontrivial surface state is the most intriguing one. Such materials demonstrate the quantum anomalous Hall effect, which manifests itself as chiral edge conduction channels that can be manipulated by switching the polarization of magnetic domains. In the present paper, we uncover the atomic structure of the bulk and the surface of Mn0.06Sb1.22Bi0.78Te3.06 in conjunction with its electronic and magnetic properties; this material is characterized by naturally formed ferromagnetic layers inside the insulating matrix, where the Fermi level is tuned to the bulk band gap. We found that in such mixed crystals septuple layers (SLs) of Mn(Bi,Sb)2Te4 form structures that feature three SLs, each of which is separated by two or three (Bi,Sb)2Te3 quintuple layers (QLs); such a structure possesses ferromagnetic properties. The surface obtained by cleavage includes terraces with different terminations. Manganese atoms preferentially occupy the central positions in the SLs and in a very small proportion can appear in the QLs, as indirectly indicated by a reshaped Dirac cone.

Fermi surface tomography.

Fermi surfaces are essential for predicting, characterizing and controlling the properties of crystalline metals and semiconductors. Angle-resolved photoemission spectroscopy (ARPES) is the only technique directly probing the Fermi surface by measuring the Fermi momenta (kF) from energy- and angular distribution of photoelectrons dislodged by monochromatic light. Existing apparatus is able to determine a number of kF -vectors simultaneously, but direct high-resolution 3D Fermi surface mapping remains problematic. As a result, no such datasets exist, strongly limiting our knowledge about the Fermi surfaces. Here we show that using a simpler instrumentation it is possible to perform 3D-mapping within a very short time interval and with very high resolution. We present the first detailed experimental 3D Fermi surface as well as other experimental results featuring advantages of our technique. In combination with various light sources our methodology and instrumentation offer new opportunities for high-resolution ARPES in the physical and life sciences.

Hidden spin-orbital texture at the [Formula: see text]-located valence band maximum of a transition metal dichalcogenide semiconductor.

Finding stimuli capable of driving an imbalance of spin-polarised electrons within a solid is the central challenge in the development of spintronic devices. However, without the aid of magnetism, routes towards this goal are highly constrained with only a few suitable pairings of compounds and driving mechanisms found to date. Here, through spin- and angle-resolved photoemission along with density functional theory, we establish how the p-derived bulk valence bands of semiconducting 1T-HfSe2 possess a local, ground-state spin texture spatially confined within each Se-sublayer due to strong sublayer-localised electric dipoles orientated along the c-axis. This hidden spin-polarisation manifests in a 'coupled spin-orbital texture' with in-equivalent contributions from the constituent p-orbitals. While the overall spin-orbital texture for each Se sublayer is in strict adherence to time-reversal symmetry (TRS), spin-orbital mixing terms with net polarisations at time-reversal invariant momenta are locally maintained. These apparent TRS-breaking contributions dominate, and can be selectively tuned between with a choice of linear light polarisation, facilitating the observation of pronounced spin-polarisations at the Brillouin zone centre for all kz. We discuss the implications for the generation of spin-polarised populations from 1T-structured transition metal dichalcogenides using a fixed energy, linearly polarised light source.

Is There a Polaron Signature in Angle-Resolved Photoemission of CsPbBr_{3}?

The formation of large polarons has been proposed as reason for the high defect tolerance, low mobility, low charge carrier trapping, and low nonradiative recombination rates of lead halide perovskites. Recently, direct evidence for large-polaron formation has been reported from a 50% effective mass enhancement in angle-resolved photoemission of CsPbBr_{3} over theory for the orthorhombic structure. We present in-depth band dispersion measurements of CsPbBr_{3} and GW calculations, which lead to similar effective masses at the valence band maximum of 0.203±0.016 m_{0} in experiment and 0.226 m_{0} in orthorhombic theory. We argue that the effective mass can be explained solely on the basis of electron-electron correlation and large-polaron formation cannot be concluded from photoemission data.

Direct Spectroscopic Evidence of Magnetic Proximity Effect in MoS2 Monolayer on Graphene/Co.

A magnetic field modifies optical properties and provides valley splitting in a molybdenum disulfide (MoS2) monolayer. Here we demonstrate a scalable approach to the epitaxial synthesis of MoS2 monolayer on a magnetic graphene/Co system. Using spin- and angle-resolved photoemission spectroscopy we observe a magnetic proximity effect that causes a 20 meV spin-splitting at the Γ̅ point and canting of spins at the K̅ point in the valence band toward the in-plane direction of cobalt magnetization. Our density functional theory calculations reveal that the in-plane spin component at K̅ is localized on Co atoms in the valence band, while in the conduction band it is localized on the MoS2 layer. The calculations also predict a 16 meV spin-splitting at the Γ̅ point and 8 meV K̅-K'¯ valley asymmetry for an out-of-plane magnetization. These findings suggest control over optical transitions in MoS2 via Co magnetization. Our estimations show that the magnetic proximity effect is equivalent to the action of the magnetic field as large as 100 T.

Ultrafast Thermalization Pathways of Excited Bulk and Surface States in the Ferroelectric Rashba Semiconductor GeTe.

A large Rashba effect is essential for future applications in spintronics. Particularly attractive is understanding and controlling nonequilibrium properties of ferroelectric Rashba semiconductors. Here, time- and angle-resolved photoemission is utilized to access the ultrafast dynamics of bulk and surface transient Rashba states after femtosecond optical excitation of GeTe. A complex thermalization pathway is observed, wherein three different timescales can be clearly distinguished: intraband thermalization, interband equilibration, and electronic cooling. These dynamics exhibit an unconventional temperature dependence: while the cooling phase speeds up with increasing sample temperature, the opposite happens for interband thermalization. It is demonstrated how, due to the Rashba effect, an interdependence of these timescales on the relative strength of both electron-electron and electron-phonon interactions is responsible for the counterintuitive temperature dependence, with spin-selection constrained interband electron-electron scatterings found both to dominate dynamics away from the Fermi level, and to weaken with increasing temperature. These findings are supported by theoretical calculations within the Boltzmann approach explicitly showing the opposite behavior of all relevant electron-electron and electron-phonon scattering channels with temperature, thus confirming the microscopic mechanism of the experimental findings. The present results are important for future applications of ferroelectric Rashba semiconductors and their excitations in ultrafast spintronics.

Emergence of Fermi arcs due to magnetic splitting in an antiferromagnet.

The Fermi surface plays an important role in controlling the electronic, transport and thermodynamic properties of materials. As the Fermi surface consists of closed contours in the momentum space for well-defined energy bands, disconnected sections known as Fermi arcs can be signatures of unusual electronic states, such as a pseudogap1. Another way to obtain Fermi arcs is to break either the time-reversal symmetry2 or the inversion symmetry3 of a three-dimensional Dirac semimetal, which results in formation of pairs of Weyl nodes that have opposite chirality4, and their projections are connected by Fermi arcs at the bulk boundary3,5-12. Here, we present experimental evidence that pairs of hole- and electron-like Fermi arcs emerge below the Neel temperature (TN) in the antiferromagnetic state of cubic NdBi due to a new magnetic splitting effect. The observed magnetic splitting is unusual, as it creates bands of opposing curvature, which change with temperature and follow the antiferromagnetic order parameter. This is different from previous theoretically considered13,14 and experimentally reported cases15,16 of magnetic splitting, such as traditional Zeeman and Rashba, in which the curvature of the bands is preserved. Therefore, our findings demonstrate a type of magnetic band splitting in the presence of a long-range antiferromagnetic order that is not readily explained by existing theoretical ideas.

Mn-Rich MnSb2 Te4 : A Topological Insulator with Magnetic Gap Closing at High Curie Temperatures of 45-50 K.

Ferromagnetic topological insulators exhibit the quantum anomalous Hall effect, which is potentially useful for high-precision metrology, edge channel spintronics, and topological qubits.  The stable 2+ state of Mn enables intrinsic magnetic topological insulators. MnBi2 Te4 is, however, antiferromagnetic with 25 K Néel temperature and is strongly n-doped. In this work, p-type MnSb2 Te4 , previously considered topologically trivial, is shown to be a ferromagnetic topological insulator for a few percent Mn excess. i) Ferromagnetic hysteresis with record Curie temperature of 45-50 K, ii) out-of-plane magnetic anisotropy, iii) a 2D Dirac cone with the Dirac point close to the Fermi level, iv) out-of-plane spin polarization as revealed by photoelectron spectroscopy, and v) a magnetically induced bandgap closing at the Curie temperature, demonstrated by scanning tunneling spectroscopy (STS), are shown. Moreover, a critical exponent of the magnetization ß ≈ 1 is found, indicating the vicinity of a quantum critical point. Ab initio calculations reveal that Mn-Sb site exchange provides the ferromagnetic interlayer coupling and the slight excess of Mn nearly doubles the Curie temperature. Remaining deviations from the ferromagnetic order open the inverted bulk bandgap and render MnSb2 Te4 a robust topological insulator and new benchmark for magnetic topological insulators.

Atomic and Electronic Structure of a Multidomain GeTe Crystal.

Renewed interest in the ferroelectric semiconductor germanium telluride was recently triggered by the direct observation of a giant Rashba effect and a 30-year-old dream about a functional spin field-effect transistor. In this respect, all-electrical control of the spin texture in this material in combination with ferroelectric properties at the nanoscale would create advanced functionalities in spintronics and data information processing. Here, we investigate the atomic and electronic properties of GeTe bulk single crystals and their (111) surfaces. We succeeded in growing crystals possessing solely inversion domains of ∼10 nm thickness parallel to each other. Using HAADF-TEM we observe two types of domain boundaries, one of them being similar in structure to the van der Waals gap in layered materials. This structure is responsible for the formation of surface domains with preferential Te-termination (∼68%) as we determined using photoelectron diffraction and XPS. The lateral dimensions of the surface domains are in the range of ∼10-100 nm, and both Ge- and Te-terminations reveal no reconstruction. Using spin-ARPES we establish an intrinsic quantitative relationship between the spin polarization of pure bulk states and the relative contribution of different terminations, a result that is consistent with a reversal of the spin texture of the bulk Rashba bands for opposite configurations of the ferroelectric polarization within individual nanodomains. Our findings are important for potential applications of ferroelectric Rashba semiconductors in nonvolatile spintronic devices with advanced memory and computing capabilities at the nanoscale.

Contrast Reversal in Scanning Tunneling Microscopy and Its Implications for the Topological Classification of SmB6.

SmB6 has recently attracted considerable interest as a candidate for the first strongly correlated topological insulator. Such materials promise entirely new properties such as correlation-enhanced bulk bandgaps or a Fermi surface from spin excitations. Whether SmB6 and its surface states are topological or trivial is still heavily disputed however, and a solution is hindered by major disagreement between angle-resolved photoemission (ARPES) and scanning tunneling microscopy (STM) results. Here, a combined ARPES and STM experiment is conducted. It is discovered that the STM contrast strongly depends on the bias voltage and reverses its sign beyond 1 V. It is shown that the understanding of this contrast reversal is the clue to resolving the discrepancy between ARPES and STM results. In particular, the scanning tunneling spectra reflect a low-energy electronic structure at the surface, which supports a trivial origin of the surface states and the surface metallicity of SmB6 .

Band Renormalization of Blue Phosphorus on Au(111).

Most recently, theoretical calculations predicted the stability of a novel two-dimensional phosphorus honeycomb lattice named blue phosphorus. Here, we report on the growth of blue phosphorus on Au(111) and unravel its structural details using diffraction, microscopy and theoretical calculations. Most importantly, by utilizing angle-resolved photoemission spectroscopy we identify its momentum-resolved electronic structure. We find that Au(111) breaks the sublattice symmetry of blue phosphorus leading to an orbital-dependent band renormalization upon the formation of a (4 × 4) superstructure. Notably, the semiconducting two-dimensional phosphorus realizes its valence band maximum at 0.9 eV binding energy, however, shifted in momentum space due to the substrate-induced band renormalization.

High-temperature quantum oscillations of the Hall resistance in bulk Bi2Se3.

Helically spin-polarized Dirac fermions (HSDF) in protected topological surface states (TSS) are of high interest as a new state of quantum matter. In three-dimensional (3D) materials with TSS, electronic bulk states often mask the transport properties of HSDF. Recently, the high-field Hall resistance and low-field magnetoresistance indicate that the TSS may coexist with a layered two-dimensional electronic system (2DES). Here, we demonstrate quantum oscillations of the Hall resistance at temperatures up to 50 K in nominally undoped bulk Bi2Se3 with a high electron density n of about 2·1019 cm-3. From the angular and temperature dependence of the Hall resistance and the Shubnikov-de Haas oscillations we identify 3D and 2D contributions to transport. Angular resolved photoemission spectroscopy proves the existence of TSS. We present a model for Bi2Se3 and suggest that the coexistence of TSS and 2D layered transport stabilizes the quantum oscillations of the Hall resistance.

Observation of hidden atomic order at the interface between Fe and topological insulator Bi2Te3.

To realize spintronic devices based on topological insulators (TIs), well-defined interfaces between magnetic metals and TIs are required. Here, we characterize atomically precisely the interface between the 3d transition metal Fe and the TI Bi2Te3 at different stages of its formation. Using photoelectron diffraction and holography, we show that after deposition of up to 3 monolayers Fe on Bi2Te3 at room temperature, the Fe atoms are ordered at the interface despite the surface disorder revealed by our scanning-tunneling microscopy images. We find that Fe occupies two different sites: a hollow adatom deeply relaxed into the Bi2Te3 quintuple layers and an interstitial atom between the third (Te) and fourth (Bi) atomic layers. For both sites, our core-level photoemission spectra and density-functional theory calculations demonstrate simultaneous chemical bonding of Fe to both Te and Bi atoms. We further show that upon deposition of Fe up to a thickness of 20 nm, the Fe atoms penetrate deeper into the bulk forming a 2-5 nm interface layer containing FeTe. In addition, excessive Bi is pushed down into the bulk of Bi2Te3 leading to the formation of septuple layers of Bi3Te4 within a distance of ∼25 nm from the interface. Controlling the magnetic properties of the complex interface structures revealed by our work will be of critical importance when optimizing the efficiency of spin injection in TI-based devices.

Topological quantum phase transition from mirror to time reversal symmetry protected topological insulator.

Topological insulators constitute a new phase of matter protected by symmetries. Time-reversal symmetry protects strong topological insulators of the Z2 class, which possess an odd number of metallic surface states with dispersion of a Dirac cone. Topological crystalline insulators are merely protected by individual crystal symmetries and exist for an even number of Dirac cones. Here, we demonstrate that Bi-doping of Pb1-x Sn x Se (111) epilayers induces a quantum phase transition from a topological crystalline insulator to a Z2 topological insulator. This occurs because Bi-doping lifts the fourfold valley degeneracy and induces a gap at [Formula: see text], while the three Dirac cones at the [Formula: see text] points of the surface Brillouin zone remain intact. We interpret this new phase transition as caused by a lattice distortion. Our findings extend the topological phase diagram enormously and make strong topological insulators switchable by distortions or electric fields.Transitions between topological phases of matter protected by different symmetries remain rare. Here, Mandal et al. report a quantum phase transition from a topological crystalline insulator to a Z2 topological insulator by doping Bi into Pb1-x Sn x Se (111) thin films.